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Robust optical readout and characterization of nuclear spin transitions in nitrogen-vacancy ensembles in diamond

Andrey Jarmola, Ilja Fescenko, Víctor M. Acosta, Marcus W. Doherty, Fredrik K. Fatemi, Tony Ivanov, Dmitry Budker, Vladimir S. Malinovsky

Published Jan 1, 2020• 20 citations
OpenAlex

Abstract

Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperature T yielding d|Q|/dT=-35.0(2) Hz/K at T=297 K. The temperature and magnetic field dependencies reported here are important for quantum sensing applications such as rotation sensing and potentially for applications in quantum information processing.

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arXiv:1807.08100•Physical review. B./Physical review. B•Sep 18, 2020•20 citations
Nuclear spin ensembles in diamond are promising candidates for quantum sensing applications, including rotation sensing. Here we perform a characterization of the optically detected nuclear-spin transitions associated with the 14N nuclear spin within diamond nitrogen vacancy (NV) centers. We observe nuclear-spin-dependent fluorescence with the contrast of optically detected 14N nuclear Rabi oscillations comparable to that of the NV electron spin. Using Ramsey spectroscopy, we investigate the temperature and magnetic-field dependence of the nuclear spin transitions in the 77.5-420 K and 350-675 G range, respectively. The nuclear quadrupole coupling constant Q was found to vary with temperature T yielding d|Q|/dT=-35.0(2) Hz/K at T=297 K. The temperature and magnetic field dependencies reported here are important for quantum sensing applications such as rotation sensing and potentially for applications in quantum information processing.
Precision measurements based on optically detected nuclear magnetic resonance offer exquisite sensitivity to absolute shifts in spin transition frequencies, with potential applications in fundamental physics experiments and inertial sensing. We investigate 13C nuclear spins in diamond as a candidate system for solid-state implementations, which hold the promise for high-fidelity readout of large numbers of coherent nuclear spins in millitesla or lower magnetic fields. We demonstrate a technique that allows for both optical polarization and readout of large ensembles of ~10^{16} polarized nuclear spins. Our method takes advantage of state-selective Landau-Zener transitions under microwave frequency sweeping, which bidirectionally transfer spin polarization between Nitrogen-Vacancy (NV) electron spins and remote 13C nuclear spins. Using natural isotopic abundance diamonds with nitrogen densities of ~0.5-10 ppm, we perform optically-detected 13C Ramsey spectroscopy and realize a nuclear-spin-dependent fluorescence contrast exceeding 0.5% peak-to-peak. We observe nuclear spin dephasing times T2*~2 ms that only modestly improve with homonuclear dipolar decoupling, indicating that they are limited by the longitudinal spin relaxation of nearby NV electron spins. We study the magnetic field dependence of the optical readout and find comparable contrast and dephasing times for magnetic fields in the range 8-20 mT. Our method can be interpreted as a type of repetitive readout, where each NV center optically reads out the spin state of ~10^2 nuclei before nuclear spins depolarize.
Nitrogen vacancy (NV-) color centers in diamond are a prime candidate for use in quantum information devices, owing to their spin-1 ground state, straightforward optical initialization and readout, and long intrinsic coherence times in a room-temperature solid. While the 13C nuclear spin is often a dominant source of magnetic noise, we observe transitions between electron-nuclear hyperfine states of NV- centers in 99% 13C diamond that are robust to decoherence. At magnetic field strengths ranging from 550 - 900 G, these transitions are observable by optically detected magnetic resonance (ODMR), and exhibit linewidths narrowed by factors as high as ~130 at room temperature over typical electron-type transitions observed from this spin system. We anticipate the use of these decoherence-protected transitions, in combination with dynamical decoupling methods, for storage of quantum information.
Temperature Sensitivity of 14NV^{14}\mathrm{NV}14NV and 15NV^{15}\mathrm{NV}15NV Ground State Manifolds
We measure electron and nuclear spin transition frequencies in the ground state of nitrogen-vacancy (NV) centers in diamond for two nitrogen isotopes (14NV^{14}\mathrm{NV}14NV and 15NV^{15}\mathrm{NV}15NV) over temperatures ranging from 77 K to 400 K. Measurements are performed using Ramsey interferometry and direct optical readout of the nuclear and electron spins. We extract coupling parameters QQQ (for 14NV^{14}\mathrm{NV}14NV), DDD, A∣∣A_{||}A∣∣​, A⊥A_{\perp}A⊥​, γe/γnγ_e/γ_nγe​/γn​, and their temperature dependences for both isotopes. The temperature dependences of the nuclear-spin transitions within the ms=0m_s = 0ms​=0 spin manifold near room temperature are found to be +0.52(1) ppm/K for 14NV^{14}\mathrm{NV}14NV (∣mI=−1>↔∣mI=+1>|m_I=-1> \leftrightarrow |m_I=+1>∣mI​=−1>↔∣mI​=+1>) and -1.1(1) ppm/K for 15NV^{15}\mathrm{NV}15NV (∣mI=−1/2>↔∣mI=+1/2>|m_I=-1/2> \leftrightarrow |m_I=+1/2>∣mI​=−1/2>↔∣mI​=+1/2>). An isotopic shift in the zero-field splitting parameter DDD between 14NV^{14}\mathrm{NV}14NV and 15NV^{15}\mathrm{NV}15NV is measured to be ∼\sim∼ 120 kHz. Residual transverse magnetic fields are observed to shift the nuclear spin transition frequencies, especially for 15NV^{15}\mathrm{NV}15NV. We have precisely determined the set of parameters relevant for the development of nuclear-spin-based diamond quantum sensors with greatly reduced sensitivity to environmental factors.
Nuclear spins in certain solids couple weakly to their environment, making them attractive candidates for quantum information processing and inertial sensing. When coupled to the spin of an optically active electron, nuclear spins can be rapidly polarized, controlled, and read via lasers and radio-frequency (rf) fields. Possessing typical coherence times of several milliseconds at room temperature, nuclear spins hosted by a nitrogen-vacancy center in diamond are thus intriguing systems to observe how classical physical rotation at quantum timescales affects a quantum system. In this work, we demonstrate optical nuclear-spin polarization and rapid quantum control of nuclear spins in a diamond physically rotating at 1kHz1\phantom{\rule{0.16em}{0ex}}\mathrm{kHz}1kHz, faster than the nuclear-spin coherence time. Free from the need to maintain strict field alignment, we are able to measure and control nuclear spins in the presence of a large, time-varying magnetic field that makes an angle of more than ${100}^{\ensuremath{\circ}}$ to the nitrogen-lattice vacancy axis. The field induces spin mixing between the electron and nuclear states of the qubits, decoupling them from oscillating rf fields. We are able to demonstrate that coherent spin state control is possible at any point of the rotation. We combine continuous dynamical decoupling with feed-forward control to eliminate decoherence induced by imperfect mechanical rotation. Our work liberates a previously inaccessible degree of freedom of the NV nuclear spin, unlocking new approaches to quantum control and rotation sensing.
The nitrogen-vacancy (NV) center in diamond has been found to be a powerful tool for various sensing applications. In particular, in ensemble-based sensors, the main ``workhorse'' so far has been optically detected electron resonance. Utilization of the nuclear spin has the potential to significantly improve sensitivity in rotation and magnetic field sensors. Ensemble-based sensors consume a substantial amount of power, leading to noticeable heating of the diamond and thus requiring an understanding of temperature-related shifts. In this paper, we provide a detailed study of the temperature shift of the hyperfine components of the NV center.